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Distinct Efficacies of Interlayers in Tailoring Polyamide Nanofiltration Membrane Performance for Organic Micropollutant Removal: Dependent on Substrate Characteristics

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ENVIRONMENTAL SCIENCE & TECHNOLOGY 2024年第31期58卷 14022-14033页

作者： Cheng, Peng Liu, Yanling Wei, Xinxin Fan, Kaiming Xia, Shengji Tongji Univ Tongji Adv Membrane Technol Ctr State Key Lab Pollut Control & Resources Reuse Shanghai 200092 Peoples R China Tongji Univ Key Lab Yangtze River Water Environm Minist Educ Shanghai 200092 Peoples R China

Interlayered thin-film nanocomposite (TFN) membranes have shown the potential to boost nanofiltration performance for water treatment applications including the removal of organic micropollutants (OMPs). However, the effects of substrates have been overlooked when exploiting and evaluating the efficacy of certain kinds of interlayers in tailoring membrane performance. Herein, a series of TFN membranes were synthesized on different porous substrates with identical interlayers of metal-organic framework nanosheets. It was revealed that the interlayer introduction could narrow but not fully eliminate the difference in the properties among the polyamide layers formed on different substrates, and the membrane performance variation was prominent in distinct aspects. For substrates with small pore sizes exerting severe water transport hindrance, the introduced interlayer mainly enhanced membrane water permeance by affording the gutter effect, while it could be more effective in reducing membrane pore size by improving the interfacial polymerization platform and avoiding PA defects when using a large-pore-size substrate. By matching the selected substrates and interlayers well, superior TFN membranes were obtained with simultaneously higher water permeance and OMP rejections compared to three commercial membranes. This study helps us to objectively understand interlayer efficacies and attain performance breakthroughs of TFN membranes for more efficient water treatment.

关键词： nanofiltration thin-film nanocomposite interlayers porous substrates organic micropollutants

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Unravelling relationships between fluorescence spectra, molecular weight distribution and hydrophobicity fraction of dissolved organic matter in municipal wastewater

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CHEMOSPHERE 2022年第Part3期308卷 136359页

作者： Ji, Wen-Xiang Tian, Ye-Chao Li, Ai-min Gu, Xiao-Ming Sun, Hong-Fang Cai, Min-Hui Shen, Shan-Qi Zuo, Yan-Ting Li, Wen-Tao Nanjing Univ Sch Environm State Key Lab Pollut Control & Resources Reuse Nanjing 210023 Peoples R China

The characteristics of dissolved organic matter (DOM) in the influent and secondary effluent from 6 municipal wastewater treatment plants (WWTPs) were investigated with a size exclusion chromatogram (SEC) coupled with multiple detectors to simultaneously detect ultraviolet absorbance, fluorescence, dissolved organic carbon (DOC) and dissolved organic nitrogen (DON) as a function of molecular weight (MW). The SEC chromatograms showed that biopolymers (>6 kDa) and humic substances (0.5-6 kDa) comprised the significant fraction in the influent, while humic substances became the abundant proportion in the secondary effluent. Direct linkages between MW distribution and hydrophobicity of DOM in the secondary effluent were further explored via SEC analysis of XAD resin fractions. DON and DOC with different hydrophobicity exhibited significantly distinct MW distribution, indicating that it was improper to consider DOC as a surrogate for DON. Different from DOC, the order of averaged MW in terms of DON was hydrophobic neutral transphilic neutral > hydrophobic acid > transphilic acid > hydrophilic fraction. Fluorescence spectral properties exhibited a significant semi-quantitative correlation with MW and hydrophobicity of DOC, with Pearson's coefficients of -0.834 and 0.754 (p < 0.01) for biopolymer and humic substances. Meanwhile, regional fluorescence proportion was demonstrated to indicate the MW and hydrophobicity properties of DON at the semi-quantitative level. The fluorescence excitation-emission matrix (EEM) could be explored to provide a rapid estimation of MW distribution and hydrophobic/hydrophilic proportion of DOC and DON in WWTPs.

关键词： Dissolved organic matter Size exclusion chromatography Molecular weight distribution Hydrophobic/hydrophilic fractionation Fluorescence property

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Enhancing separation performance of thin film nanocomposite membranes by self-etching of polydopamine-modified calcium carbonate during interfacial polymerization process

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JOURNAL OF MEMBRANE SCIENCE 2025年 715卷

作者： Wei, Xinxin Wang, Xuelin Fan, Kaiming Liu, Yanling Xia, Shengji Tongji Univ Adv Membrane Technol Ctr State Key Lab Pollut Control & Resources Reuse Shanghai 200092 Peoples R China Tongji Univ Key Lab Yangtze River Water Environm Minist Educ Shanghai 200092 Peoples R China Shanghai Inst Pollut Control & Ecol Secur Shanghai Peoples R China

The acid-accepting and gas-generating properties, along with the formation of extensive nanovoids, make CaCO3 nanoparticles attractive as sacrificial nanofillers for fabricating thin-film composite (TFN) nanofiltration membranes. However, challenges such as severe agglomeration and limited acid etching efficiency of the nanoparticles hinder the pursuit of superior membrane performance. In this study, the dispersion and compatibility of CaCO3 nanoparticles within the membrane matrix were improved by modifying them with a polydopamine (PDA) coating. The abundant phenolic hydroxyl groups of PDA enhanced the hydrophilicity and negative charges of membrane surface. Additionally, the PDA capsule increased the etching extent of the CaCO3 nanoparticles by improving the nanoparticle dispersion and generating additional acid, which created sufficient water channels within the polyamide layer. It was demonstrated that incorporating 45 mu g/cm2 of PDA-modified CaCO3 nanoparticles doubled the water permeance to 16.7 LMH/bar, while maintaining a low molecular weight cut-off of 249 Da and achieving rejections over 90 % for five types of per- and polyfluorinated substances. The PDA modification also overcame the membrane stability issue caused by the agglomerated CaCO3 nanoparticles. This study provides a novel strategy for applying properly modified self-etching nanofillers in TFN membrane development, showing great potential for water treatment applications.

关键词： Calcium carbonate Dopamine Thin-film nanocomposite membrane Acid etching per- and polyfluorinated substances

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Ecological risks in downstream lakes exacerbated by the three Gorges reservoir

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ECOLOGICAL INDICATORS 2025年 170卷

作者： Chen, Xinxin Guo, Yaxin Zhang, Junhong Han, Xiao Huang, Weiya Yue, Yao South Cent Minzu Univ Coll Resources & Environm Sci Key Lab Resources Convers & Pollut Control State Ethn Affairs Commiss Wuhan 430074 Peoples R China Nanjing Univ Sch Environm State Key Lab Pollut Control & Resource Reuse Nanjing 210023 Peoples R China Wuhan Blue Sky & Green Field Consulting Design Co Wuhan 430070 Peoples R China

River regulation through reservoir construction is one of the greatest challenges to the natural flow state and ecological health of river systems globally. The Three Gorges Dam (TGD), the largest dam in the world, has been in operation since 2003 to regulate water resources downstream. However, most of the current research on the TGD compares the post-2003 hydrologic patterns downstream of the TGD with the pre-2003 hydrologic patterns and lacks direct evidence of the TGD impacts on the downstream areas. In this paper, the ecological impacts of TGD on downstream large lakes are explored in terms of hydrological alteration degree, biodiversity, connectivity, and ecological surplus and ecological deficit by building a 1/2-dimensional nested model to simulate the hydrological processes with and without the TGD from 2008 to 2011. The results showed that (1) TGD storage led to a decrease in the number of high pulses at downstream stations, resulting in wetland degradation in the riverine region;(2) the SI (Shannon's diversity index) based on hydrological calculations became smaller, indicating that the downstream biodiversity showed a decreasing trend;(3) the diversion ratio and the confluence ratio of Dongting Lake and the Yangtze River decreased at the same time, and the connectivity decreased, which would lead to an increase in the degree and frequency of droughts during the dry season;(4) after the regulation of the TGD, the low-risk months were transformed into medium-risk months of the Dongting Lake basin, indicating a deterioration of the ecological situation in this region. The study demonstrates that the construction of the TGD has exacerbated downstream water stress, while the degradation of wetlands and the reduction in biodiversity highlight the heightened pressure on ecological and environmental protection downstream of the TGD. The results of this study provide necessary information for evaluating the impact of the TGD project on large lakes downstream and

关键词： Hydrological alteration Connectivity Biodiversity Ecological surplus and ecological deficit

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Hydrophobic Biodegradable Hyperbranched Copolymers with Excellent Marine Diatom Resistance

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BIOMACROMOLECULES 2022年第10期23卷 4327-4338页

作者： Si, Chunying Hu, Guoming Jiang, Wei Sun, Ping Cao, Jingjing Ji, Ruixiang Li, Ai -Min Zhang, Quanxing Nanjing Univ State Key Lab Pollut Control & Resources Reuse Sch Environm Nanjing 210023 Peoples R China

As the utilization of degradable polymer coatings increased, the accompanying trade-off between good degradability and high-efficiency antidiatom adhesion due to their hydrophobic nature remains unresolved. The study presents a new hydrophobic surface-fragmenting coating consisting of degradable hyper-branched polymers (hereafter denoted as h-LLA(x)) synthesized by reversible complexation-mediated copolymerization with isobornyl acrylate (IBOA) and divinyl-functional oligomeric poly(L-lactide) (OLLA-V-2), both derived from biomass, that exhibited superior resistance (similar to 0 cell mm(-2)) to marine diatom Navicula incerta (N. incerta) attachment with higher OLLA content. The combined impact of the microscale hollow semisphere micelles that self-assembled degradable hyperbranched copolymers and hydrolysis-driven self-renewable surfaces following immersion in seawater may account for the remarkable resistance of h-LLA(x) coatings against N. incerta. Detailed investigations were conducted across multiple perspectives, from hydrolytic degradation to broad-spectrum antibacterial attachment to ecotoxicity assessment. The excellent features of high resistance to marine diatoms and bacterial attachment, degradability, and environmental friendliness make the as-prepared h-LLA(x) coatings widely sought after for antifouling coating applications.

关键词： Hydrophobicity

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A hybrid fuel cell for water purification and simultaneously electricity generation

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Frontiers of Environmental Science & Engineering 2023年第1期17卷 121-132页

作者： Yujun Zhou Qinghua Ji Chengzhi Hu Huijuan Liu Jiuhui Qu Key Laboratory of Drinking Water Science and Technology Research Center for Eco-Environmental SciencesChinese Academy of SciencesBeijing 100085China Center for Water and Ecology State Key Joint Laboratory of Environment Simulation and Pollution ControlSchool of EnvironmentTsinghua UniversityBeijing 100084China Jiangsu Key Laboratory of Chemical Pollution Control and Resources Reuse School of Environmental and Biological EngineeringNanjing University of Science and TechnologyNanjing 210094China

The development of highly efficient energy conversion technologies to extract energy from wastewater is urgently needed,especially in facing of increasing energy and environment ***,we successfully fabricated a novel hybrid fuel cell with BiOCl-NH_(4)PTA as *** polyoxometalate(NH_(4)PTA)act as the acceptor of photoelectrons and could retard the recombination of photogenerated electrons and holes,which lead to superior photocatalytic *** utilizing BiOCl-NH_(4)PTA as photocatalysts and Pt/C air-cathode,we successfully constructed an electron and mass transfer enhanced photocatalytic hybrid fuel cell with flow-through field(F-HFC).In this novel fuel cell,dyes and biomass could be directly degraded and stable power output could be *** 87%of dyes could be degraded in 30 min irradiation and nearly 100%removed within 90 *** current density could reach up to~267.1μA/cm^(2);with maximum power density(Pmax)of~16.2μW/cm^(2) with Rhodamine B as organic pollutant in *** power densities were 9.0μW/cm^(2),12.2μW/cm^(2),and 13.9μW/cm^(2) when using methyl orange(MO),glucose and starch as substrates,*** hybrid fuel cell with BiOCl-NH_(4)PTA composite fulfills the purpose of decontamination of aqueous organic pollutants and synchronous electricity ***,the novel design cell with separated photodegradation unit and the electricity generation unit could bring potential practical application in water purification and energy recovery from wastewater.

关键词： Flow-through field Hybrid fuel cell Polyoxometalates Water purification Electricity generation

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Novel simulation of aqueous total nitrogen and phosphorus concentrations in Taihu Lake with machine learning

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ENVIRONMENTAL RESEARCH 2022年第PartB期204卷 111940-111940页

作者： Lu, Hao Yang, Liuyan Fan, Yifan Qian, Xin Liu, Tong Nanjing Univ Sch Environm State Key Lab Pollut Control & Resources Reuse Nanjing 210023 Peoples R China

This study demonstrates the utility of internal nutrient loads as an additional parameter to improve the performance of machine learning models in predicting the temporal variations of aqueous TN and TP concentrations in Taihu Lake, a large shallow lake. Internal loads, as a potential input parameter for machine learning models, were estimated using a mass balance calculation. The results showed that between 2011 and 2018 the maximum monthly internal loads of nitrogen and phosphorus in Taihu Lake were 4200 t and 178 t, respectively. Monthly changes in the aqueous TN and TP concentrations of Taihu Lake did not correlate significantly with inflow loads whereas the correlations with estimated internal loads were positive and significant. Long short-term memory (LSTM), random forest (RF), and gradient boosting regression tree (GBRT) models were built, and for all of them the inclusion of internal loads in the input parameters improved their performance. LSTM model III, whose input parameters included both inflow loads and internal loads, had the best performance, based on a testing root mean square error of 0.11 mg TN/L and 0.017 mg TP/L. A 28 % decrease in the annual aqueous TP concentration in Taihu Lake in 2018 simulated by LSTM model III was achieved by lowering the average water level from 3.29 m to 2.99 m, suggesting a possible strategy to control the TP concentration in the lake. In summary, our study showed that aqueous TN and TP concentrations in shallow lakes can be simulated using machine learning, with LSTM models outperforming RF and GBRT models;in these models, internal loads should be included as an input parameter. Additionally, our study identified the water level as an important factor affecting the aqueous TP concentration in Taihu Lake.

关键词： Internal load Long short-term memory Random forest Gradient boosting regression tree Water level

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Simultaneous and long-term effective immobilization of lead, cadmium and arsenic in multi-contaminated soil by ferrihydrite-supported animal-derived biochar

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JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING 2023年第3期11卷

作者： Hong, Chengyi Zhang, Jichen Liu, Tingran Teng, Wei Fu, Rongbing Qiu, Yuping Tongji Univ Shanghai Inst Pollut Control & Ecol Secur State Key Lab Pollut Control & Resources Reuse Dept Environm SciColl Environm Sci & Engn Shanghai 200092 Peoples R China

The multi-contaminants of cationic Pb/Cd and anionic As in soils is difficult to simultaneously immobilize by common chemical amendments. Here, a novel ferrihydrite-supported animal-derived biochar (FAB) was prepared and added to pristine Pb/Cd/As-contaminated soil for incubation of 150 days. The amendment using FAB elevated soil pH and reduced soil electric conductivity and the release of soil dissolved organic carbon. After the addition of 3 %w/w FAB (FAB3 %), the bioavailability of Pb, Cd, and As decreased to 9.2, 57.5, and 7.6 mg/kg, respectively, which were 96 %, 47 %, and 36 % lower than that of the control soil (CK). The exchangeable Pb and Cd and specifically sorbed As were transformed into residual Pb, carbonate- and Fe-Mn oxide-bound Cd, and well-crystallized Fe-Al oxide-bound As, respectively. The diversity of soil bacterial community increased after FAB treatment. Dynamic leaching and first-order attenuation simulation experiments showed that FAB3 % can decrease the leachable heavy metal(loid)s to negligible concentration in real soil within 3-7 years, whereas that in CK soil was around 12 years. X-Ray adsorption near edge structure analysis showed that FAB immobilized heavy metal(loid)s in soil by forming pyromorphite coprecipitate with Pb(II), ion exchange between Cd(II) and Ca(II) in the hydroxyapatite component, and complexation between the ferrihydrite component and As(V).

关键词： Animal-derived biochar Ferrihydrite Heavy metal(loid)s Soil remediation XANES

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Mechanism of polyhydroquinone coating iron/copper oxides for enhanced catalytic activity

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CHEMICAL ENGINEERING JOURNAL 2022年 427卷 131007-131007页

作者： Yang, Zhen Ma, Yan Zhou, Qing Nanjing Univ Sch Environm State Key Lab Pollut Control & Resources Reuse Nanjing 210023 Peoples R China

In this study, Polyhydroquinone (PHQ) coated eight kinds of iron/copper oxides (CuO, Cu2O, Fe3O4, Fe2O3, CCuFe2O4, T-CuFe2O4, 3R-CuFeO2, 2H-CuFeO2) to enhance their catalytic activity. As evidenced by the characterization results, PHQ was coated at Cu(I), Cu(II), and Fe(II) sites rather than Fe(III) sites by forming metalorganic complexes at the catalyst surface. These results were supported by catalytic experiments of Persulfate (PS) activation for 1,4-dioxane degradation. Based on the normalized pseudo-first-order kinetics constant, PHQ enhanced iron/copper sites in the order of Cu(I) > Fe(II) approximate to Cu(II). Interestingly, in contrast to the general agreement, the Hard and Soft Acids and Bases (HSAB) Principle indicated that the benzene ring (soft base) rather than the phenolic hydroxyl group (hard base) was the reactive site between Fe/Cu and PHQ. Six of the above eight iron/copper oxides (CuO, Cu2O, Fe3O4, C-CuFe2O4, 3R-CuFeO2, 2H-CuFeO2) displayed improved catalytic performance. The other two catalysts (Fe2O3 and T-CuFe2O4) showed no improvement in activity after PHQ coating. Among all the catalysts, PHQ/2H-CuFeO2 showed the best catalytic performance, which was also able to activate Hydrogen peroxide (HP) and Peroxymonosulfate (PMS) for 1,4-dioxane degradation by a radical pathway. However, radical process caused the decomposition of PHQ at the catalyst surface, leading to a dramatic drop (from 100% to approximately 30%) in catalyst activity. In contrast, PHQ/2H-CuFeO2 activated PS by a nonradical pathway where Cu(III) was likely responsible for 1,4-dioxane degradation. PHQ/2H-CuFeO2 was more stable after activating PS.

关键词： Persulfate Hydrogen peroxide Peroxymonosulfate Bimetallic iron-copper oxides Polyhydroquinone Enhanced catalyst

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Screening of indicator pharmaceuticals and personal care products in landfill leachates: a case study in Shanghai, China

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Frontiers of Environmental Science & Engineering 2023年第9期17卷 245-256页

作者： Xiping Kan Xia Yu Wentao Zhao Shuguang Lyu Shuying Sun Gang Yu Qian Sui State Environmental Protection Key Laboratory of Environmental Risk Assessment and Control on Chemical Process School of Resources and Environmental EngineeringEast China University of Science and TechnologyShanghai 200237China State Key Laboratory of Pollution Control and Resource Reuse College of Environmental Science and EngineeringTongji UniversityShanghai 200092China Advanced Interdisciplinary Institute of Environment and Ecology Beijing Normal University at ZhuhaiZhuhai 519087China Shanghai Institute of Pollution Control and Ecological Security Shanghai 200092China

Identifying potential sources of pharmaceuticals and personal care products(PPCPs)in the environment is critical for the effective control of PPCP *** leachate is an important source of PPCPs in water;however,it has barely been involved in source apportionment due to the lack of indicator-PPCPs(i-PPCPs)in landfill *** study provides the first systematic framework for identifying i-PPCPs for landfill leachates based on the wide-scope target monitoring of *** number of target PPCPs increased from<20 in previous studies to 68 in the present ***-nine PPCPs were detected,with median concentrations in leachate samples ranging from below the method quantification limit(MQL)to 41μg/L,and 19 of them were rarely reported previously.A total of 29 target compounds were determined to be PPCPs of high concern by principal component analysis according to multiple criteria,including occurrence,exposure potential,and ecological *** with source-specificity and representativeness analysis,erythromycin,gemfibrozil,and albendazole showed a significant difference in their occurrence in leachate compared to other potential sources(untreated and treated municipal wastewater and livestock wastewater)and correlated with total PPCP concentrations;these were recommended as i-PPCPs for *** screening procedure can be used to develop a sophisticated source apportionment method to identify sources of PPCPs from adjacent landfills.

关键词： Landfill leachates PPCPs Indicator Screening criteria Source-specificity

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